The Mechanism of Activation of a [NiFe]-Hydrogenase by Electrons, Hydrogen, and Carbon Monoxide

Activation of the oxidized inactive state (termed Unready or Niu*) of the [NiFe]-hydrogenase from Allochromatium vinosum requires removal of an unidentified oxidizing entity [O], produced by partial reduction of O2. Dynamic electrochemical kinetic studies, subjecting enzyme molecules on an electrode...

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Bibliographic Details
Published in:Journal of the American Chemical Society 2005-05, Vol.127 (18), p.6595-6604
Main Authors: Lamle, Sophie E, Albracht, Simon P. J, Armstrong, Fraser A
Format: Article
Language:English
Subjects:
Biological and medical sciences
Carbon Monoxide - chemistry
Carbon Monoxide - metabolism
Carbon Monoxide - pharmacology
Chromatiaceae - enzymology
Electrochemistry
Enzyme Activation
Fundamental and applied biological sciences. Psychology
Hydrogen - chemistry
Hydrogen - metabolism
Hydrogenase - antagonists & inhibitors
Hydrogenase - chemistry
Hydrogenase - metabolism
Kinetics
Molecular biophysics
Oxidation-Reduction
Oxygen - chemistry
Oxygen - metabolism
Physical chemistry in biology
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Summary:Activation of the oxidized inactive state (termed Unready or Niu*) of the [NiFe]-hydrogenase from Allochromatium vinosum requires removal of an unidentified oxidizing entity [O], produced by partial reduction of O2. Dynamic electrochemical kinetic studies, subjecting enzyme molecules on an electrode to sequences of potential steps and gas injections, establish the order of events in an otherwise complex sequence of reactions that involves more than one intermediate retaining [O] or its redox equivalent; fast and reversible electron transfer precedes the rate-determining step which is followed by a reaction with H2, or the inhibitor CO, that renders the reductive activation process irreversible.
ISSN:0002-7863
1520-5126
DOI:10.1021/ja0424934